应用于同步辐射光电离质谱的原位催化高压反应器研制

doi:10.3969/j.issn.0253-2778.2020.07.002

中国科学技术大学学报 ›› 2020, Vol. 50 ›› Issue (7): 880-886.DOI: 10.3969/j.issn.0253-2778.2020.07.002

应用于同步辐射光电离质谱的原位催化高压反应器研制

余圣圣，文武，许鸣皋，杨玖重，毕海林，王旭迪，齐飞，潘洋

1.中国科学技术大学国家同步辐射实验室，安徽合肥 230029；2.合肥工业大学机械工程学院，安徽合肥 230009；

收稿日期:2020-04-14 修回日期:2020-06-01 接受日期:2020-06-01 出版日期:2020-07-31 发布日期:2020-06-01
通讯作者: 潘洋
作者简介:余圣圣，男，1995年生，硕士.研究方向：同步辐射应用.E-mail:yss0318@mail.ustc.edu.cn
基金资助:
国家自然科学基金（91845203，91945302,92045301）资助.

Development of an in situ high-pressure catalytic reactor for synchrotron radiation photoionization mass spectrometry

YU Shengsheng, WEN Wu, XU Minggao, YANG Jiuchong, BI Hailin, WANG Xudi, QI Fei, PAN Yang

1.National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China; 2.School of Mechanical Engineering, Hefei University of Technology, Hefei 230009, China; 3.School of Mechanical Engineering, Shanghai Jiaotong University, Shanghai 200240

Received:2020-04-14 Revised:2020-06-01 Accepted:2020-06-01 Online:2020-07-31 Published:2020-06-01

摘要/Abstract

摘要： 研制了一种可与同步辐射真空紫外光电离质谱结合的原位催化高压反应器.通过在高压反应管末端加工锥形微孔进行一次取样，再经过石英喷嘴二次取样的方法与质谱相连，使反应器工作压力范围可从常压至3.6 MPa.设计上采用了气体动力学理论计算以及COMSOL Multiphysics软件仿真，并通过实验测量对仿真结果进行了验证.同时，在近工况不同压力下对二甲醚羰基化催化制备乙酸甲酯反应进行了原位质谱研究，发现实时获得的乙酸甲酯选择性随反应压力增加显著提高.该原位催化高压反应器的成功研制将有助于深入开展高压下气固相催化反应机理研究.

关键词: 高压催化, 同步辐射, 光电离质谱, COMSOL Multiphysics仿真, 二甲醚羰基化

Abstract: An in situ high-pressure catalytic reactor which can be coupled with synchrotron radiation vacuum ultraviolet photoionization mass spectrometry was developed. A tapered micro orifice was designed at the top of the high-pressure reaction tube for the first sampling, along with a quartz nozzle downstream connected with the mass spectrometry for the second sampling. Thus, the working pressure range of the reactor could reach from atmosphere to 3.6 MPa. In this design, gas dynamics theory and COMSOL Multiphysics software were applied for simulation, and the simulation results were verified by experimental measurements. The dimethyl ether (DME) carbonylation to methyl acetate reaction under different pressures near working conditions was studied by in situ mass spectrometry simultaneously. It was found that the selectivity of methyl acetate obtained in real time increased significantly with the increase of reaction pressure. The development of the in situ high-pressure catalytic reactor will be helpful to further study gas-solid catalytic reaction mechanism under high pressure.

Key words: high-pressure catalysis, synchrotron radiation, photoionization mass spectrometry, COMSOL Multiphysics simulation, DME carboxylation

中图分类号:

TH843

余圣圣，文武，许鸣皋，杨玖重，毕海林，王旭迪，齐飞，潘洋. 应用于同步辐射光电离质谱的原位催化高压反应器研制[J]. 中国科学技术大学学报, 2020, 50(7): 880-886.

YU Shengsheng, WEN Wu, XU Minggao, YANG Jiuchong, BI Hailin, WANG Xudi, QI Fei, PAN Yang. Development of an in situ high-pressure catalytic reactor for synchrotron radiation photoionization mass spectrometry[J]. Journal of University of Science and Technology of China, 2020, 50(7): 880-886.

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应用于同步辐射光电离质谱的原位催化高压反应器研制

Development of an in situ high-pressure catalytic reactor for synchrotron radiation photoionization mass spectrometry

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